Abstract. Concern in recent decades about human impacts on Earth's climate has led to the need for improved and expanded measurement capabilities of greenhouse gases in the atmosphere. In this paper we describe in detail an in situ trace gas analyser based on Fourier Transform Infrared (FTIR) spectroscopy that is capable of simultaneous and continuous measurements of carbon dioxide (CO 2 ), methane (CH 4 ), carbon monoxide (CO), nitrous oxide (N 2 O) and 13 C in CO 2 in air with high precision. High accuracy is established by reference to measurements of standard reference gases. Stable water isotopes can also be measured in undried airstreams. The analyser is automated and allows unattended operation with minimal operator intervention. Precision and accuracy meet and exceed the compatibility targets set by the World Meteorological Organisation -Global Atmosphere Watch for baseline measurements in the unpolluted troposphere for all species except 13 C in CO 2 .The analyser is mobile and well suited to fixed sites, tower measurements, mobile platforms and campaign-based measurements. The isotopic specificity of the opticallybased technique and analysis allows its application in isotopic tracer experiments, for example in tracing variations of 13 C in CO 2 and 15 N in N 2 O. We review a number of applications illustrating use of the analyser in clean air monitoring, micrometeorological flux and tower measurements, mobile measurements on a train, and soil flux chamber measurements.

Abstract. We thoroughly evaluate the performance of a multi-species, in situ Fourier transform infrared (FTIR) analyser with respect to high-accuracy needs for greenhouse gas monitoring networks. The in situ FTIR analyser is shown to measure CO2, CO, CH4 and N2O mole fractions continuously, all with better reproducibility than the inter-laboratory compatibility (ILC) goals, requested by the World Meteorological Organization (WMO) for the Global Atmosphere Watch (GAW) programme. Simultaneously determined δ13CO2 reaches reproducibility as good as 0.03‰. Second-order dependencies between the measured components and the thermodynamic properties of the sample, (temperature, pressure and flow rate) and the cross sensitivities among the sample constituents are investigated and quantified. We describe an improved sample delivery and control system that minimises the pressure and flow rate variations, making post-processing corrections for those quantities non-essential. Temperature disequilibrium effects resulting from the evacuation of the sample cell are quantified and improved by the usage of a faster temperature sensor. The instrument has proven to be linear for all measured components in the ambient concentration range. The temporal stability of the instrument is characterised on different time scales. Instrument drifts on a weekly time scale are only observed for CH4 (0.04 nmol mol−1 day−1) and δ13CO2 (0.02‰ day−1). Based on 10 months of continuously collected quality control measures, the long-term reproducibility of the instrument is estimated to ±0.016 μmol mol−1 CO2, ±0.03‰ δ13CO2, ±0.14 nmol mol−1 CH4, ±0.1 nmol mol−1 CO and ±0.04 nmol mol−1 N2O. We propose a calibration and quality control scheme with weekly calibrations of the instrument that is sufficient to reach WMO-GAW inter-laboratory compatibility goals.

Abstract. We present a local-scale atmospheric inversion framework to estimate the location and rate of methane (CH4) and carbon dioxide (CO2) releases from point sources. It relies on mobile near-ground atmospheric CH4 and CO2 mole fraction measurements across the corresponding atmospheric plumes downwind of these sources, on high-frequency meteorological measurements, and on a Gaussian plume dispersion model. The framework exploits the scatter of the positions of the individual plume cross sections, the integrals of the gas mole fractions above the background within these plume cross sections, and the variations of these integrals from one cross section to the other to infer the position and rate of the releases. It has been developed and applied to provide estimates of brief controlled CH4 and CO2 point source releases during a 1-week campaign in October 2018 at the TOTAL experimental platform TADI in Lacq, France. These releases typically lasted 4 to 8 min and covered a wide range of rates (0.3 to 200 g CH4/s and 0.2 to 150 g CO2/s) to test the capability of atmospheric monitoring systems to react fast to emergency situations in industrial facilities. It also allowed testing of their capability to provide precise emission estimates for the application of climate change mitigation strategies. However, the low and highly varying wind conditions during the releases added difficulties to the challenge of characterizing the atmospheric transport over the very short duration of the releases. We present our series of CH4 and CO2 mole fraction measurements using instruments on board a car that drove along roads ∼50 to 150 m downwind of the 40 m × 60 m area for controlled releases along with the estimates of the release locations and rates. The comparisons of these results to the actual position and rate of the controlled releases indicate ∼10 %–40 % average errors (depending on the inversion configuration or on the series of tests) in the estimates of the release rates and ∼30–40 m errors in the estimates of the release locations. These results are shown to be promising, especially since better results could be expected for longer releases and under meteorological conditions more favorable to local-scale dispersion modeling. However, the analysis also highlights the need for methodological improvements to increase the skill for estimating the source locations.

Abstract. We present a local-scale atmospheric inversion framework to estimate the location and rate of methane (CH4) and carbon dioxide (CO2) releases from point sources. It relies on mobile near-ground atmospheric CH4 and CO2 mole fraction measurements across the corresponding atmospheric plumes downwind the sources, on high-frequency meteorological measurements, and a Gaussian plume dispersion model. It exploits the spread of the positions of individual plume cross-sections and the integrals of the gas mole fractions above the background within these plume cross-sections to infer the position and rate of the releases. It has been developed and applied to provide estimates of brief controlled CH4 and CO2 point source releases during a one-week campaign in October 2018 at the TOTAL's experimental platform TADI in Lacq, France. These releases lasted typically 4 to 8 minutes and covered a wide range of rates (0.3 to 200 gCH4/s and 0.2 to 150 gCO2/s) to test the capability of atmospheric monitoring systems to react fast to emergency situations in industrial facilities. It also allowed testing their capability to provide precise emission estimates for the application of climate change mitigation strategies. However, the low and highly varying wind conditions during the releases added difficulties to the challenge of characterizing the atmospheric transport over the very short duration of the releases. We present our series of measurements of CH4 and CO2 mole fractions using instruments onboard a car that drives along the roads ~50 to 150 m downwind the 40 m × 60 m area of controlled releases for each of the releases and the results from the inversions of the release locations and rates. The comparisons of these results to the actual position and rate of the controlled release indicate a 20 %–30 % average error on the release rates and a ~30–40 m errors in the estimates of the release locations. These results are shown to be promising especially since better results could be expected for longer releases and under meteorological conditions more favorable to local scale dispersion modeling.

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Abstract. This study presents two methods for estimating methane emissions from a waste water treatment plant (WWTP) along with results from a measurement campaign at a WWTP in Valence, France. These methods, chamber measurements and tracer release, rely on Fourier transform infrared spectroscopy and cavity ring-down spectroscopy instruments. We show that the tracer release method is suitable for quantifying facility-and some process-scale emissions, while the chamber measurements provide insight into individual process emissions. Uncertainties for the two methods are described and discussed. Applying the methods to CH 4 emissions of the WWTP, we confirm that the open basins are not a major source of CH 4 on the WWTP (about 10 % of the total emissions), but that the pretreatment and sludge treatment are the main emitters. Overall, the waste water treatment plant is representative of an average French WWTP.

We thoroughly evaluate the performance of a multi-species, in-situ FTIR analyser with respect to high accuracy needs for greenhouse gas monitoring networks. The in-situ FTIR analyser measures CO₂, CO, CH₄ and N₂O mole fractions continuously, all with better reproducibility than requested by the WMO-GAW inter-laboratory compatibility (ILC) goal. Simultaneously determined δ¹³CO₂ reaches reproducibility as good as 0.03‰. This paper focuses on the quantification of residual dependencies between the measured components and the thermodynamic properties of the sample as well as the cross-sensitivities among the sample constituents. The instrument has proven to be linear for all components in the ambient range. The temporal stability of the instrument was investigated by 10 months of continuously collected quality control measures. Based on these measures we conclude that for moderately stable laboratory conditions weekly calibrations of the instrument are sufficient to reach WMO-GAW ILC goals

Concern in recent decades about human impacts on Earth's climate has led to the need for improved and expanded measurement capabilities for greenhouse gases in the atmosphere. In this paper we describe in detail an in situ trace gas analyser based on Fourier Transform Infrared (FTIR) spectroscopy that is capable of simultaneous and continuous measurements of carbon dioxide (CO₂), methane (CH₄), carbon monoxide (CO), nitrous oxide (N₂O) and ¹³C in CO₂ in air with high precision and accuracy. Stable water isotopes can also be measured in undried airstreams. The analyser is automated and allows unattended operation with minimal operator intervention. Precision and accuracy meet and exceed the compatibility targets set by the World Meteorological Organisation – Global Atmosphere Watch Programme for baseline measurements in the unpolluted troposphere for all species except ¹³C in CO₂. <br><br> The analyser is mobile and well suited to fixed sites, tower measurements, mobile platforms and campaign-based measurements. The isotopic specificity of the optically-based technique and analysis allows application of the analyser in isotopic tracer experiments, for example ¹³C in CO₂ and ¹⁵N in N₂O. We review a number of applications illustrating use of the analyser in clean air monitoring, micrometeorological flux and tower measurements, mobile measurements on a train, and soil flux chamber measurements